Lewis acid protection turns cyanide containing [FeFe]-hydrogenase mimics into proton reduction catalysts.

ABSTRACT: Sustainable sources of hydrogen are a vital component of the envisioned energy transition. Understanding and mimicking the [FeFe]-hydrogenase provides a route to achieving this goal. In this study we re-visit a molecular mimic of the hydrogenase, the propyl dithiolate bridged complex [Fe₂(μ-pdt)(CO)₄(CN)₂]^2-, in which the cyanide ligands are tuned via Lewis acid interactions. This system provides a rare example of a cyanide containing [FeFe]-hydrogenase mimic capable of catalytic proton reduction, as demonstrated by cyclic voltammetry. EPR, FTIR, UV-vis and X-ray absorption spectroscopy are employed to characterize the species produced by protonation, and reduction or oxidation of the complex. The results reveal that biologically relevant

SUBMITTER: Redman HJ 

PROVIDER: S-EPMC8939051 | biostudies-literature | 2022 Mar

REPOSITORIES: biostudies-literature